Guo Zhaoyan, Ren Guangyuan, Jiang Congcong, Lu Xianyong, Zhu Ying, Jiang Lei, Dai Liming
Key Laboratory of Bio-inspired Smart Interfacial Science and Technology of Ministry of Education, School of Chemistry and Environment, Beihang University, Beijing 100191, People's Republic of China.
Beijing National Laboratory for Molecular Sciences, Institute of Chemistry Chinese Academy of Sciences, Beijing, 100190, P.R. China.
Sci Rep. 2015 Nov 25;5:17064. doi: 10.1038/srep17064.
A novel heteroatoms (N, P, S and Fe) quaternary-doped carbon (HQDC-X, X refers to the pyrolysis temperature) can be fabricated by directly pyrolyzing a gram-negative bacteria, S. oneidensis MR-1 as precursors at 800 °C, 900 °C and 1000 °C under argon atmosphere. These HQDC-X catalysts maintain the cylindrical shape of bacteria after pyrolysis under high temperatures, while heteroatoms including N, P, S and Fe distribute homogeneously on the carbon frameworks. As a result, HQDC-X catalysts exhibit excellent electrocatalytic activity for ORR via a dominant four-electron oxygen reduction pathway in alkaline medium, which is comparable with that of commercial Pt/C. More importantly, HQDC-X catalysts show better tolerance for methanol crossover and CO poisoning effects, long-term durability than commercial Pt/C, which could be promising alternatives to costly Pt-based electrocatalysts for ORR. The method may provide a promising avenue to develop cheap ORR catalysts from inexpensive, scalable and biological recursors.
通过在氩气气氛下,于800°C、900°C和1000°C直接热解革兰氏阴性细菌——嗜铁锰氧化还原菌MR-1作为前驱体,可制备出一种新型杂原子(N、P、S和Fe)四元掺杂碳(HQDC-X,X表示热解温度)。这些HQDC-X催化剂在高温热解后保持了细菌的圆柱形形状,而包括N、P、S和Fe在内的杂原子均匀分布在碳骨架上。因此,HQDC-X催化剂在碱性介质中通过占主导地位的四电子氧还原途径对氧还原反应表现出优异的电催化活性,这与商业Pt/C相当。更重要的是,HQDC-X催化剂对甲醇渗透和CO中毒效应表现出比商业Pt/C更好的耐受性和长期耐久性,这可能成为用于氧还原反应的昂贵Pt基电催化剂的有前途的替代品。该方法可能为从廉价、可扩展的生物前驱体开发廉价的氧还原反应催化剂提供一条有前途的途径。